CAS: Ambient Electrochemical Activation of Light Alkanes with Early Transition Metal-Oxo Species

CAS：利用早期过渡金属-氧代物质对轻质烷烃进行环境电化学活化

基本信息

批准号：
1955836
负责人：
Chong Liu
金额：
$ 45万
依托单位：
University of California-Los Angeles
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2020
资助国家：
美国
起止时间：
2020-08-01 至 2023-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1955836&HistoricalAwards=false
关键词：
CAS Ambient Electrochemical Activation Light

项目摘要

The abundant, yet widely geographically distributed, natural gas and oil resources in North America have dramatically changed the United States energy portfolio. Conversion of natural gas to useful products relies on high temperature and high pressure processes at centralized locations. Transportation of natural gas from remote sources to these central locations is often not economical. As a result, natural gas is often discarded by flaring at the well, while the oil is recovered. Natural gas, which is mostly methane, and its flaring product, carbon dioxide, are both potent greenhouse gases. Development of catalytic processes that convert natural gas into economically-transportable liquids at these well sites is very desirable. In this project, Professor Chong Liu of the University of California, Los Angeles is developing a new approach using electricity to convert light alkanes, including methane, into liquid products. Dr. Liu is studying new electrochemical catalysts and investigating the fundamental mechanisms of these reactions. Dr. Liu is actively engaged in outreach and education activities to promote engagement of students in science, technology, engineering and mathematics (STEM) disciplines. These activities include the introduction of chemistry topics to local gardeners and farmers in the Los Angeles area as well as undergraduate advising for general chemistry courses assisted by machine learning.With the funding from the Chemical Catalysis Program of the Division of Chemistry, Dr. Liu of the University of California, Los Angeles is developing a mechanistic understanding of how early transition metal-oxo species break the carbon-hydrogen bond in methane during the catalysis. A variety of electrochemical techniques in conjunction with in situ characterizations (including X-ray absorption spectroscopy) are employed to identify important transient intermediate species and determine reaction kinetics with the assistance of first-principle calculations. Also under investigation is the exploration of other molecular and materials catalysts for electrochemical conversion of light alkanes under ambient conditions. Dr. Liu takes soil samples and analyzes their composition for local gardeners and farmers, assisting the local community to develop sustainable agriculture and gardening practices. Dr. Liu is also developing a machine-learning-based platform to develop teaching strategies in general chemistry courses, to advise students on course enrollment, and, in the long run, to establish an online advising program for career development.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

北美丰富且地理分布广泛的天然气和石油资源极大地改变了美国的能源结构。天然气转化为有用产品依赖于集中地点的高温高压过程。将天然气从偏远地区运输到这些中心地点通常并不经济。因此，天然气常常因油井燃烧而被丢弃，而石油则被回收。天然气（主要成分是甲烷）及其燃烧产物二氧化碳都是强效温室气体。非常需要开发在这些井场将天然气转化为经济可运输液体的催化工艺。在这个项目中，加州大学洛杉矶分校的 Chong Liu 教授正在开发一种新方法，利用电力将包括甲烷在内的轻质烷烃转化为液体产品。刘博士正在研究新型电化学催化剂并研究这些反应的基本机制。刘博士积极参与外展和教育活动，以促进学生对科学、技术、工程和数学（STEM）学科的参与。这些活动包括向洛杉矶地区当地的园丁和农民介绍化学主题，以及为本科生提供机器学习辅助的普通化学课程建议。在化学系化学催化项目的资助下，刘博士加州大学洛杉矶分校正在研究早期过渡金属-氧物种如何在催化过程中破坏甲烷中的碳-氢键的机制。采用各种电化学技术与原位表征（包括 X 射线吸收光谱）相结合来识别重要的瞬态中间体物种，并在第一原理计算的帮助下确定反应动力学。还在研究中的还有其他分子和材料催化剂的探索，用于在环境条件下进行轻质烷烃的电化学转化。刘博士为当地园丁和农民采集土壤样本并分析其成分，协助当地社区发展可持续农业和园艺实践。刘博士还在开发一个基于机器学习的平台，以制定普通化学课程的教学策略，为学生提供课程注册建议，并从长远来看，建立一个职业发展在线咨询计划。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力优点和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

期刊论文数量（4）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Bisulfate as a redox-active ligand in vanadium-based electrocatalysis for CH 4 functionalization

硫酸氢盐作为钒基电催化 CH 4 功能化的氧化还原活性配体

DOI：
10.1039/d1cc06596c
发表时间：
2022
期刊：
Chemical Communications
影响因子：
4.9
作者：
Xiang, Danlei;Lin, Sheng-Chih;Deng, Jiao;Chen, Hao Ming;Liu, Chong
通讯作者：
Liu, Chong

Electrocatalytic Methane Functionalization with d 0 Early Transition Metals Under Ambient Conditions

环境条件下 d 0 早期过渡金属的电催化甲烷功能化

DOI：
10.1002/anie.202107720
发表时间：
2021
期刊：
Angewandte Chemie International Edition
影响因子：
0
作者：
Deng, Jiao;Lin, Sheng‐Chih;Fuller, III, Jack T.;Zandkarimi, Borna;Chen, Hao Ming;Alexandrova, Anastassia N.;Liu, Chong
通讯作者：
Liu, Chong

Ambient methane functionalization initiated by electrochemical oxidation of a vanadium (V)-oxo dimer

DOI：
10.1038/s41467-020-17494-w
发表时间：
2020-07
期刊：
Nature Communications
影响因子：
16.6
作者：
Jiao Deng;Sheng-Chih Lin;Jack T Fuller;Jesus A. Iñiguez;Danlei Xiang;Di Yang;Gary Chan;Hao Ming Che
通讯作者：
Jiao Deng;Sheng-Chih Lin;Jack T Fuller;Jesus A. Iñiguez;Danlei Xiang;Di Yang;Gary Chan;Hao Ming Che

Ag II ‐Mediated Electrocatalytic Ambient CH 4 Functionalization Inspired by HSAB Theory

Ag II — 受 HSAB 理论启发的介导电催化环境 CH 4 功能化

DOI：
10.1002/anie.202104217
发表时间：
2021
期刊：
Angewandte Chemie International Edition
影响因子：
0
作者：
Xiang, Danlei;Iñiguez, Jesus A.;Deng, Jiao;Guan, Xun;Martinez, Antonio;Liu, Chong
通讯作者：
Liu, Chong